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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: 31 August 2024 | Viewed by 16799

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Dr. Maria Manuela Silva

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Centro de Química e Departamento de Química, Universidade do Minho, Gualtar, 4710-057 Braga, Portugal
Interests: solid polymer electrolytes; natural polymers; batteries; smart windows; electrochromic devices
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Dear colleagues,

There is a growing demand for electrochemical devices, such as displays, smart windows, sensors, capacitors, fuel cells, solar cells, and batteries, all of which are becoming more and more sophisticated. These devices have to be powerful enough to meet the technological advances and the development we are witnessing today, and as such, they require an innovative vision for new materials and concepts.

Despite the potential high impact and applications for electrochemical devices, the problems with their materials’ development (electrodes, electrolytes, passivation, etc.), reliability, safety, and the possibility of integrating them into complex systems remain a clear challenge. We invite authors to submit original research and review articles that seek to address the current limitations related to some of the abovementioned challenges. We are interested in articles that explore aspects concerning novel materials, new methods for preparation and characterization, environmental friendliness, low cost, etc.

Prof. Dr. Maria Manuela Silva
Guest Editor

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Keywords

solid-state devices
batteries
electrochromic devices
smart windows
electrochemical devices

Published Papers (10 papers)

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Research

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13 pages, 3366 KiB

Open AccessArticle

ZIF-67-Derived Flexible Sulfur Cathode with Improved Redox Kinetics for High-Performance Li-S Batteries

by Chen Cheng, Hanyan Wu, Xinyang Chen, Shuiping Cai, Yingkang Tian, Xiaofei Yang and Xuejie Gao

Molecules 2024, 29(8), 1833; https://doi.org/10.3390/molecules29081833 - 17 Apr 2024

Viewed by 228

Abstract

Lithium–sulfur (Li-S) batteries have received much attention due to their high energy density and low price. In recent years, alleviating the volume expansion and suppressing the shuttle effect during the charge and discharge processes of Li-S batteries have been widely addressed. However, the slow conversion kinetics from polysulfide (LiPSs) to Li₂S₂/Li₂S still limits the application of Li-S batteries. Therefore, we designed a ZIF-67 grown on cellulose (named ZIF-67@CL) as an electrocatalyst to improve the interconversion kinetics from LiPSs to Li₂S₂/Li₂S for Li-S batteries. Based on the results of adsorption experiments of LiPSs, ZIF-67@CL and CL hosts were immersed in Li₂S₄ solution to adsorb LiPSs, and the UV-Vis test was conducted on the supernatant after adsorption. The results showed that the ZIF-67@CL had a stronger adsorption for LiPSs compared with the cellulose (CL). Furthermore, in the Li₂S nucleation tests, the fabricated cells were galvanostatically discharged to 2.06 V at 0.112 mA and then potentiostatically discharged at 2.05 V. Based on the results of Li₂S nucleation tests, the catalytic effect of ZIF-67 was further verified. As a result, the sulfur cathode used a ZIF-67 catalyst (named S/ZIF-67@CL) and delivered an initial capacity of 1346 mAh g⁻¹ at a current density of 0.2 C. Even at a high current density of 2 C, it exhibited a high-capacity performance of 1087 mAh g⁻¹ on the first cycle and maintained a capacity output of 462 mAh g⁻¹ after 150 cycles, with a Coulombic efficiency of over 99.82%. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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12 pages, 3492 KiB

Open AccessArticle

Implementation of Highly Stable Memristive Characteristics in an Organic–Inorganic Hybrid Resistive Switching Layer of Chitosan-Titanium Oxide with Microwave-Assisted Oxidation

by Dong-Hee Lee, Hamin Park and Won-Ju Cho

Molecules 2023, 28(13), 5174; https://doi.org/10.3390/molecules28135174 - 03 Jul 2023

Cited by 1 | Viewed by 903

Abstract

This study proposes a high-performance organic–inorganic hybrid memristor for the development of neuromorphic devices in the memristor-based artificial synapse. The memristor consists of a solid polymer electrolyte (SPE) chitosan layer and a titanium oxide (TiO_x) layer grown with a low-thermal-budget, microwave-assisted oxidation. The fabricated Ti/SPE–chitosan/TiO_x/Pt-structured memristor exhibited steady bipolar resistive switching (BRS) characteristics and demonstrated excellent endurance in 100-cycle repetition tests. Compared to SPE–chitosan memristors without a TiO_x layer, the proposed organic–inorganic hybrid memristor demonstrated a higher dynamic range and a higher response to pre-synaptic stimuli such as short-term plasticity via paired-pulse facilitation. The effect of adding the TiO_x layer on the BRS properties was examined, and the results showed that the TiO_x layer improved the chemical and electrical superiority of the proposed memristor synaptic device. The proposed SPE–chitosan organic–inorganic hybrid memristor also exhibited a stable spike-timing-dependent plasticity, which closely mimics long-term plasticity. The potentiation and depression behaviors that modulate synaptic weights operated stably via repeated spike cycle tests. Therefore, the proposed SPE–chitosan organic–inorganic hybrid memristor is a promising candidate for the development of neuromorphic devices in memristor-based artificial synapses owing to its excellent stability, high dynamic range, and superior response to pre-synaptic stimuli. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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14 pages, 2076 KiB

Open AccessArticle

Improving Crystallization and Stability of Perovskite Solar Cells Using a Low-Temperature Treated A-Site Cation Solution in the Sequential Deposition

by Tinghao Li, Qiu Xiong, Chongzhu Hu, Can Wang, Ni Zhang, Shui-Yang Lien and Peng Gao

Molecules 2023, 28(10), 4103; https://doi.org/10.3390/molecules28104103 - 15 May 2023

Cited by 1 | Viewed by 1497

Abstract

The two-step sequential deposition is a commonly used method by researchers for fabricating perovskite solar cells (PSCs) due to its reproducibility and tolerant preparation conditions. However, the less-than-favorable diffusive processes in the preparation process often result in subpar crystalline quality in the perovskite films. In this study, we employed a simple strategy to regulate the crystallization process by lowering the temperature of the organic-cation precursor solutions. By doing so, we minimized interdiffusion processes between the organic cations and pre-deposited lead iodide (PbI₂) film under poor crystallization conditions. This allowed for a homogenous perovskite film with improved crystalline orientation when transferred to appropriate environmental conditions for annealing. As a result, a boosted power conversion efficiency (PCE) was achieved in PSCs tested for 0.1 cm² and 1 cm², with the former exhibiting a PCE of 24.10% and the latter of 21.56%, compared to control PSCs, which showed a PCE of 22.65% and 20.69%, respectively. Additionally, the strategy increased device stability, with the cells holding 95.8% and 89.4% of the initial efficiency even after 7000 h of aging under nitrogen or 20–30% relative humidity and 25 °C. This study highlights a promising low-temperature-treated (LT-treated) strategy compatible with other PSCs fabrication techniques, adding a new possibility for temperature regulation during crystallization. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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12 pages, 4475 KiB

Open AccessArticle

In/Ga-Doped Si as Anodes for Si–Air Batteries with Restrained Self-Corrosion and Surface Passivation: A First-Principles Study

by Dongxu Wang, Tingyu Zhao and Yingjian Yu

Molecules 2023, 28(9), 3784; https://doi.org/10.3390/molecules28093784 - 27 Apr 2023

Cited by 1 | Viewed by 1243

Abstract

Silicon–air batteries (SABs) are attracting considerable attention owing to their high theoretical energy density and superior security. In this study, In and Ga were doped into Si electrodes to optimize the capability of Si-air batteries. Varieties of Si-In/SiO₂ and Si-Ga/SiO₂ atomic interfaces were built, and their properties were analyzed using density functional theory (DFT). The adsorption energies of the SiO₂ passivation layer on In- and Ga-doped silicon electrodes were higher than those on pure Si electrodes. Mulliken population analysis revealed a change in the average number of charge transfers of oxygen atoms at the interface. Furthermore, the local device density of states (LDDOS) of the modified electrodes showed high strength in the interfacial region. Additionally, In and Ga as dopants introduced new energy levels in the Si/SiO₂ interface according to the projected local density of states (PLDOS), thus reducing the band gap of the SiO₂. Moreover, the I-V curves revealed that doping In and Ga into Si electrodes enhanced the current flow of interface devices. These findings provide a mechanistic explanation for improving the practical efficiency of silicon–air batteries through anode doping and provide insight into the design of Si-based anodes in air batteries. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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18 pages, 4249 KiB

Open AccessArticle

A Novel Cathode Material Synthesis and Thermal Characterization of (1-x-y) LiCo_1/3Ti_1/3Fe_1/3PO₄, xLi₂MnPO₄, yLiFePO₄ Composites for Lithium-Ion Batteries (LIBs)

by Lu Li, Xin Min and Majid Monajjemi

Molecules 2022, 27(23), 8486; https://doi.org/10.3390/molecules27238486 - 02 Dec 2022

Cited by 1 | Viewed by 1168

Abstract

Lithium-ion batteries are known for their high efficiency for storing electrical energy, especially for hybrid vehicles. In this research, the development of mixture composites in the cathode electrode of LIBs has been discussed and designed based on ternary solid solutions. We have given a novel synthesis and method preparation of cathode electrode materials to reduce costs while increasing the efficiency and simultaneity for the future of these technologies. The major problem in the LIBs is related to LiCoO₂ as a popular cathode material that, although it has a high efficiency, is expensive and very toxic. Therefore, the usage of a lower weight of cobalt compared to the LiCoO₂ cathode material is economically advantageous for this research. Several samples of the (1-x-y) LiCo_1/3Ti_1/3Fe_1/3PO₄ xLi₂MnPO₄ and yLiFePO₄ system were synthesized via sol–gel experiments. Various stoichiometric amounts of the LiNO₃, Li₂MnPO₄, Mn (Ac)₂. 4H₂O, Co (Ac)₂.4H₂O, Ti(NO₃)₂.6H₂O and LiFePO₄ have been used for several compositions of chrome, manganese, cobalt and titanium in 28 samples of (1-x-y) LiCo_1/3Ti_1/3Fe_1/3PO₄. By using thermal characterization, five samples have been selected due to their conditions in viewpoints of capacity and cyclability as well as activation energy, which is one of the major factors. These composites exhibited fairly consistent charge/discharge curves during the electrochemical testing. From the viewpoint of the physical and chemical properties, among these samples, the Li_1.501Co_0.389Ti_0.055Fe_0.055Mn_0.501PO₄ structure has a high efficiency compared to other compositions. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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12 pages, 4580 KiB

Open AccessArticle

A Hierarchically Ordered Mesoporous-Carbon-Supported Iron Sulfide Anode for High-Rate Na-Ion Storage

by Anupriya K. Haridas, Natarajan Angulakshmi, Arul Manuel Stephan, Younki Lee and Jou-Hyeon Ahn

Molecules 2021, 26(14), 4349; https://doi.org/10.3390/molecules26144349 - 18 Jul 2021

Cited by 4 | Viewed by 2314

Abstract

Sodium-ion batteries (SIBs) are promising alternatives to lithium-based energy storage devices for large-scale applications, but conventional lithium-ion battery anode materials do not provide adequate reversible Na-ion storage. In contrast, conversion-based transition metal sulfides have high theoretical capacities and are suitable anode materials for SIBs. Iron sulfide (FeS) is environmentally benign and inexpensive but suffers from low conductivity and sluggish Na-ion diffusion kinetics. In addition, significant volume changes during the sodiation of FeS destroy the electrode structure and shorten the cycle life. Herein, we report the rational design of the FeS/carbon composite, specifically FeS encapsulated within a hierarchically ordered mesoporous carbon prepared via nanocasting using a SBA-15 template with stable cycle life. We evaluated the Na-ion storage properties and found that the parallel 2D mesoporous channels in the resultant FeS/carbon composite enhanced the conductivity, buffered the volume changes, and prevented unwanted side reactions. Further, high-rate Na-ion storage (363.4 mAh g⁻¹ after 500 cycles at 2 A g⁻¹, 132.5 mAh g⁻¹ at 20 A g⁻¹) was achieved, better than that of the bare FeS electrode, indicating the benefit of structural confinement for rapid ion transfer, and demonstrating the excellent electrochemical performance of this anode material at high rates. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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11 pages, 1639 KiB

Open AccessArticle

Nanocomposite Polymer Electrolytes of Sodium Alginate and Montmorillonite Clay

by Franciani C. Sentanin, Willian R. Caliman, Rodrigo C. Sabadini, Carla C. S. Cavalheiro, Rui F. P. Pereira, Maria M. Silva and Agnieszka Pawlicka

Molecules 2021, 26(8), 2139; https://doi.org/10.3390/molecules26082139 - 08 Apr 2021

Cited by 3 | Viewed by 1714

Abstract

Nanocomposite polymer electrolytes (NPEs) were synthesized using sodium alginate (Alg) and either sodium (SCa-3-Na⁺)- or lithium (SCa-3-Li⁺)-modified montmorillonite clays. The samples were characterized by structural, optical, and electrical properties. SCa-3-Na⁺ and SCa-3-Li⁺ clays’ X-ray structural analyses revealed peaks at 2θ = 7.2° and 6.7° that corresponded to the interlamellar distances of 12.3 and 12.8 Å, respectively. Alg-based NPEs X-ray diffractograms showed exfoliated structures for samples with low clay percentages. The increase of clay content promoted the formation of intercalated structures. Electrochemical Impedance Spectroscopy revealed that Alg-based NPEs with 5 wt% of SCa-3-Na⁺ clay presented the highest conductivity of 1.96 × 10⁻² S/cm², and Alg with 10 wt% of SCa-3-Li⁺ showed conductivity of 1.30 × 10⁻² S/cm², both measured at 70 °C. From UV-Vis spectroscopy, it was possible to infer that increasing concentration of clay promoted a decrease of the samples’ transmittance and, consequently, an increase of their reflectance. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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13 pages, 11262 KiB

Open AccessArticle

Ionogels Obtained by Thiol-Ene Photopolymerization—Physicochemical Characterization and Application in Electrochemical Capacitors

by Agnieszka Marcinkowska, Piotr Gajewski, Katarzyna Szcześniak, Mariola Sadej and Aneta Lewandowska

Molecules 2021, 26(3), 758; https://doi.org/10.3390/molecules26030758 - 02 Feb 2021

Cited by 6 | Viewed by 2716

Abstract

Flexible ionogels with good mechanical properties were obtained in situ by thiol-ene photopolymerization of trimethylolpropane tris(3-mercaptopropionate) (TMPTP) and 1,3,5-triallyl-1,3,5-triazine-2,4,6(1H,3H,5H)-trione (TATT) (with C=C: SH ratio 1:1) in four imidazolium ionic liquids (1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide—EMImNTf₂, 1-ethyl-3-methylimidazolium trifluoromethanesulfonate-EMImOTf, 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide-BMImNTf₂, and 1-butyl-3-methylimidazolium trifluoromethanesulfonate—BMImOTf) used in the range 50 to 70 wt.%. The mechanical and electrochemical properties of obtained ionogels were examined. Ionogels with ionic liquids (ILs) with NTf₂⁻ anion are more puncture resistant than with OTf⁻ anion. Moreover, ionogels with the NTF₂⁻ anion have better electrochemical properties than those with the OTf⁻ anion. Although it should be noted that ionogels with the EMIm⁺ cation have a higher conductivity than the BMIm⁺. This is connected with intermolecular interactions between polymer matrix and IL related to the polarity of IL described by the Kamlet-Taft parameters. These parameters influence the morphology of the polymer matrix (as shown by the SEM micrograph), which is formed by interconnected polymer spheres. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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Review

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27 pages, 2369 KiB

Open AccessReview

A Comprehensive Review of In Situ Measurement Techniques for Evaluating the Electro-Chemo-Mechanical Behaviors of Battery Electrodes

by Hainan Jiang, Jie Chen, Xiaolin Li, Zhiyao Jin, Tianjun Chen, Jiahui Liu and Dawei Li

Molecules 2024, 29(8), 1873; https://doi.org/10.3390/molecules29081873 (registering DOI) - 19 Apr 2024

Abstract

The global production landscape exhibits a substantial need for efficient and clean energy. Enhancing and advancing energy storage systems are a crucial avenue to optimize energy utilization and mitigate costs. Lithium batteries are the most effective and impressive energy utilization system at present, with good safety, high energy density, excellent cycle performance, and other advantages, occupying most of the market. However, due to the defects in the electrode material of the battery itself, the electrode will undergo the process of expansion, stress evolution, and electrode damage during electro-chemical cycling, which will degrade battery performance. Therefore, the detection of property changes in the electrode during electro-chemical cycling, such as the evolution of stress and the modulus change, are useful for preventing the degradation of lithium-ion batteries. This review presents a current overview of measurement systems applied to the performance detection of batteries’ electrodes, including the multi-beam optical stress sensor (MOSS) measurement system, the digital image correlation (DIC) measurement system, and the bending curvature measurement system (BCMS), which aims to highlight the measurement principles and advantages of the different systems, summarizes a part of the research methods by using each system, and discusses an effective way to improve the battery performance. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

37 pages, 527 KiB

Open AccessReview

Development on Solid Polymer Electrolytes for Electrochemical Devices

by Li Ping Teo, Mohd Hamdi Buraidah and Abdul Kariem Arof

Molecules 2021, 26(21), 6499; https://doi.org/10.3390/molecules26216499 - 28 Oct 2021

Cited by 33 | Viewed by 3921

Abstract

Electrochemical devices, especially energy storage, have been around for many decades. Liquid electrolytes (LEs), which are known for their volatility and flammability, are mostly used in the fabrication of the devices. Dye-sensitized solar cells (DSSCs) and quantum dot sensitized solar cells (QDSSCs) are also using electrochemical reaction to operate. Following the demand for green and safer energy sources to replace fossil energy, this has raised the research interest in solid-state electrochemical devices. Solid polymer electrolytes (SPEs) are among the candidates to replace the LEs. Hence, understanding the mechanism of ions’ transport in SPEs is crucial to achieve similar, if not better, performance to that of LEs. In this paper, the development of SPE from basic construction to electrolyte optimization, which includes polymer blending and adding various types of additives, such as plasticizers and fillers, is discussed. Full article

(This article belongs to the Special Issue Materials for Emerging Electrochemical Devices)

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